Moving bed reactor for processing three phase flows

ABSTRACT

A moving bed reactor is provided that can allow facilitate performing a reaction involving a three-phase flow under co-axial flow conditions for the solid and liquid portions of the three phase flow, while the gas portion of the three-phase flow is exposed to the solids under radial flow conditions. Methods for using such a moving bed reactor to perform a reaction, such as upgrading of a feed to distillate products, are also provided.

CROSS REFERENCE TO RELATED APPLICATIONS

This application claims priority to U.S. Provisional Ser. No. 62/865,562filed Jun. 24, 2019, which is herein incorporated by reference in itsentirety.

FIELD

Systems and methods are provided for processing a three phase flow in amoving bed reactor.

BACKGROUND

Moving bed reactors are a type of reactor that is potentially suitablefor reactions where a fluid phase is exposed to catalyst and/or othersolid particles at specified temperature and pressure conditions. Movingbed reactors provide an advantage due to the movement of the solidparticles. Because the solid particles flow within the reactor, it isrelatively easy to withdraw catalyst from a moving bed reactor on aperiodic basis to regenerate the catalyst.

Although moving bed reactors can facilitate catalyst regeneration,transfer of multiple phases between moving bed reactors can presentdifficulties. In particular, moving bed reactors are not conventionallyused in situations where a three phase, e.g., gas/liquid/solid,co-current flow is transferred from a first moving bed reactor to asecond moving bed reactor. Because each phase of the three-phase flowhas different flow properties, attempting to transfer a three-phase flowby conventional methods can result in uneven distribution of one or moreflow phases. Such uneven distribution can lead to substantially reducedactivity, temperature spikes, increased catalyst deactivation, and/orvarious other poor performance characteristics. Additionally,conventional methods of transferring a three-phase flow can suffer fromlimits on the ability to independently control the input flow rate ofeach phase into the reactor.

One option for overcoming the difficulties with managing co-current flowin a moving bed reactor is to use a counter-current flow reactor, wherethe direction of travel for the solid particles is the opposite of thedirection of travel for the fluid phases. U.S. Pat. Nos. 4,968,409 and5,916,529 provide examples of moving bed reactors designed forcounter-current flow. The reactors include a distributor thatcorresponds to a cone for guiding the catalyst particles into a pipe asthe catalyst moves down through the reactor. The cone distributorincludes openings to allow gas to pass through the cone. The conedistributor also includes liquid conduits to transfer fluid from areservoir up to the catalyst in the cone distributor. While acounter-current flow reactor can handle a three-phase flow, managing thethree-phase flow is difficult. For example, the flow rates for eachphase need to be balanced to avoid flooding of the reactor.Additionally, the residence time for contact between the liquid and thecatalyst particles is relatively high, so reactions requiring a shortcontact time between the liquid and the solid phases are not suitablefor this type of counter-current reactor configuration.

European Patent Application EP 0552457 describes another example of acounter-current moving bed reactor configuration.

U.S. Pat. Nos. 7,371,915 and 7,414,167 describe co-current moving bedreactor systems for conversion of oxygenates to propylene. Because theconversion reaction converts low molecular weight oxygenates topropylene, liquid is not formed in the reactors.

U.S. Pat. No. 8,323,476 describes moving bed hydroprocessing reactorsfor hydroprocessing of liquid feeds. The amount of hydrogen introducedinto the reactors is limited so that a continuous liquid phase ismaintained within the hydroprocessing reactors. The liquid is contactedwith the solids in a radial flow configuration.

U.S. Pat. No. 5,849,976 describes a moving bed solid catalysthydrocarbon alkylation process. The reaction zone is operated at liquidphase conditions.

U.S. Pat. No. 9,162,205 describes a co-current moving bed reactor systemfor contacting fluids with adsorbent particles. Due to the nature of anadsorbent/desorbent system, maldistribution of fluid flow within thereactor may lead to reduced performance, but does not otherwise resultin problems due to excessive reaction of fluids with catalyst particles.

U.S. Patent Application Publication 2017/0137342 describes multi-phaseseparators for use in producing oxygenates and olefins fromhydrocarbons. The multi-phase separators are described as being suitablefor use in moving bed reactors.

What is needed are systems and methods to enable transfer of aco-current three-phase flow from one moving bed reactor to anothermoving bed reactor when performing reactions where it is desirable tocontrol contact time of fluids with catalyst while also managing flowuniformity. This can include having the ability to separate athree-phase flow so that each phase can be separately introduced at acontrolled rate. This can further include introducing each phase in amanner that results in substantially uniform mixing of the phases.

SUMMARY

In an aspect, a moving bed reactor is provided. The reactor includes anannular outer volume, an annular solids volume inside the annular outervolume, a first central conduit inside of the annular solids volume, andan inner central conduit inside the first central conduit. The annularsolids volume can include a plurality of perforations providing vaporcommunication between the annular outer volume and the first centralconduit. The reactor can further include a central gas opening in fluidcommunication with the outer annular volume. The reactor can furtherinclude a plurality of solids inlet conduits in solids flowcommunication with the annular solids volume. The reactor can furtherinclude one or more distributor plates comprising distributor plateconcave volumes, a plurality of the distributor plate concave volumesbeing arranged around each of the solids inlet conduits. Eachdistributor plate concave volume can include one or more orificesproviding fluid communication between each distributor plate concavevolume and the annular solids volume. The reactor can further include aplurality of liquid inlet conduits in fluid communication with thedistributor plate concave volumes. The reactor can further include a gasexit conduit in fluid communication with the inner central volume. Thereactor can further include a liquid exit conduit in fluid communicationwith the outer central volume. Additionally, the reactor can include asolids exit volume in solids flow communication with a bottom of thesolids annular volume. The solids exit volume can further include astripping gas inlet and a stripping gas outlet. The stripping gas outletcan provide fluid communication with the outer central volume.

In some aspects, the one or more distributor plates can include aplurality of exit surfaces separating the distributor plate concavevolumes from the annular solids volume. In such aspects, the one or moreorifices can provide fluid communication between each concave volume andthe annular solids volume through an exit surface. In such aspects, theplurality of exit surfaces can be oriented at an angle of 15° to 45°relative to a plane defined by at least one interface between the one ormore solids inlet conduits and the solids volume.

In another aspect, a method for operating a moving bed reactor isprovided. The method can include passing solid particles into an annularsolids volume of a moving bed reactor through a plurality of solidsinlet conduits. The solid particles can form a plurality of cones at anangle of repose for the solid particles within the annular solidsvolume. The method can further include passing a liquid feed into theannular solids volume. At least a portion of the liquid feed can impingeon the plurality of cones formed by the solid particles. The method canfurther include contacting the solid particles with a gas feed bypassing the gas feed from an outer annular volume, through the annularsolids volume, through a first central conduit, and into an innercentral conduit. The method can further include moving the solidparticles and a liquid effluent through the annular solids volume into asolids exit volume. The method can further include stripping the liquideffluent from the solid particles by passing a stripping gas through thesolids exit volume and into the first central conduit.

In some aspects, passing the liquid feed into the annular solids volumecan include introducing the liquid feed into a plurality of concavevolumes in a distributor plate. The plurality of concave volumes can bearranged around each of the plurality of solids inlet conduits. Eachconcave volume can include one or more orifices, the one or moreorifices providing fluid communication between the plurality of concavevolumes and the annular solids volume via a plurality of exit surfaces.In such aspects, the liquid feed can be passed through the one or moreorifices into the annular solids volume. In such aspects, the pluralityof exit surfaces can be oriented at an angle of 15° to 45° relative to aplane defined by at least one interface between the plurality of solidsinlet conduits and the annular solids volume.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 shows a side view of an example of a feed distribution apparatus.

FIG. 2 shows additional details for portions of the feed distributionapparatus in FIG. 1.

FIG. 3 shows a bottom view of the feed distribution apparatus shown inFIG. 1.

FIG. 4 shows a side view an example of a moving bed reactor.

FIG. 5 shows a top view of the moving bed reactor shown in FIG. 4.

DETAILED DESCRIPTION

All numerical values within the detailed description and the claimsherein are modified by “about” or “approximately” the indicated value,and take into account experimental error and variations that would beexpected by a person having ordinary skill in the art.

Overview

In various aspects, a feed distribution apparatus is provided forintroducing a three-phase flow into a moving bed reactor that isoperated under co-current flow conditions. The feed distributionapparatus can allow for separate introduction of liquid and solids in amanner that allows for even distribution of liquid within the solids.The gas portion of the flow can be introduced in any of a variety ofconvenient manners for distributing gas into a liquid or solid flow.

The distribution apparatus allows for efficient and/or substantiallyeven distribution of a co-current axial liquid flow in a solid particleflow based on the relative angle of introduction for the liquid and thesolid particles. The solid particles can be introduced into the reactorby allowing the particles to drop under gravitational pull. The conduitdropping the particles can also be narrower than the portion of thereactor that is receiving the particles. This can result in the solidparticles forming a cone based on the angle of repose for the solidparticles. The liquid can then be introduced at a plurality of locationsaround the cone. The distribution channels for introducing the liquidcan be angled at the exit surface, so that the liquid has a lateralvelocity component. Introducing the liquid with a lateral velocitycomponent can facilitate mixing of the liquid with the solid particles.However, even though the liquid initially has a lateral velocitycomponent, a substantial portion of the liquid travels axially with thecatalyst through substantially the full length of the reactor prior todisengagement of the majority of the liquid from the solids. The gas ina three-phase flow can be contacted with the solid and liquid in anaxial flow manner, a radial flow manner, or in any other convenientmanner that allows for a desired distribution pattern.

It is noted that the distributor apparatus can work in conjunction withmethods for separating a three-phase flow as the flow exits from themoving bed reactor. By separating the three-phase flow into gas, liquid,and solid components, the components can be re-combined in a subsequentmoving bed stage using the distributor apparatus. The separation of thefluid phases from the catalyst flow can be effective for separating 95mol % or more of the hydrocarbons in the effluent from the catalystflow.

One example of a suitable method for separating the three-phase flowinto gas, liquid, and solid components can be to use a stripping gas incombination with concentric pipes to allow for separate capture of thegas and liquid. For example, the stripping gas can be passed through thesolid particles in a solids exit volume, prior to the conduit forallowing solids to exit from the reactor. This can cause any liquids andgases entrained with the solid particles to be driven out of the solidsexit volume and into a separate volume, such as an outer pipe of a pairof concentric pipes. The wall between the inner pipe and the outer pipecan include protected openings, such as bubble caps, that allowtransport of gas from the outer pipe to the inner pipe while minimizingtransport of liquids. The liquids can instead accumulate at the bottomof the outer pipe and exit from openings that can be accessed when theaccumulated liquid level is sufficiently high.

An example of a type of reaction that can benefit from a moving bedreactor that can manage co-current contact of a three-phase flow isconversion of oxygenates and/or olefins to naphtha and/or distillateboiling range products. Conversion of oxygenates to olefins is anexothermic process. Oligomerization of olefins to form higher molecularweight olefins is also an exothermic process. Managing heat duringconversion of oxygenates and oligomerization of olefins generated fromoxygenate conversion can pose significant challenges in a fixed bedreactor environment. Using a plurality of moving bed reactors canmitigate or minimize such heat management difficulties. For example, aplurality of moving bed reactors can be used to perform the conversionand oligomerization reactions. The reactors can be sized and/oroperating conditions can be selected so that the amount of temperatureincrease across a single reactor is less than a target value, such ashaving a temperature rise of 85° C. (˜150° F.) or less across a reactor,or 75° C. or less, or 60° C. or less. An initial feed, which may onlycorrespond to a gas phase feed of oxygenates and light olefins, can thenbe passed into the first reactor. The plurality of moving bed reactorscan then be used to facilitate substantially complete conversion ofoxygenates as well as oligomerization of the resulting olefins to adesired degree. This can allow, for example, for conversion of an oxygenfeed (optionally also including light olefins) to distillate boilingrange products while avoiding excessive heating within any singlereactor.

Another benefit of using a plurality of moving bed reactors foroxygenate conversion and olefin oligomerization is the ability to reduceor minimize catalyst deactivation. Without being bound by any particulartheory, it is believed that there are two primary modes of catalystdeactivation for the zeotype catalysts used in oxygenate conversion andolefin oligomerization. One type of deactivation is due to cokeformation on the catalyst. As coke accumulates, it is believed thatactive sites can be blocked, resulting in lower catalyst activity.Fortunately, such coke can be removed by regeneration at hightemperature, which can restore a substantial portion (such as up to all)of the activity loss due to coke formation.

In a fixed bed catalyst environment, removal of coke from catalyst canonly occur during dedicated regeneration periods. In between suchregeneration periods, the primary option for extending run length in afixed bed reactor to a commercially desirable level is to build a largercatalyst bed. At the start of an oxygenate conversion process, thecatalyst near the top of the bed performs most of the oxygenateconversion. This results in coking of the catalyst. As cokingdeactivates the catalyst near the top of the bed, catalyst at locationsfarther down in the bed performs an increasing percentage of theoxygenate conversion. Thus, the depth of the fixed bed can be increasedso that the run length between regeneration steps is at a desirablelevel.

Although creating a larger fixed bed can be effective for overcomingdifficulties due to coke formation, such increases in the size of afixed bed can actually increase another type of deactivation. Withoutbeing bound by any particular theory, it is believed that a second typeof catalyst deactivation can be due to steaming of the catalyst, or inother words exposing the catalyst to water at elevated temperatures.

In addition to forming olefins, the oxygenate conversion reactiongenerates a substantial amount of water. For example, if methanol isused as the oxygenate feed, two moles of water are generated for eachmole of ethene produced by the oxygenate conversion reaction. In a fixedbed environment, at the beginning of an oxygenate conversion reaction,the catalyst near the top of the catalyst bed can perform substantiallyall of the oxygenate conversion. This results in creation of water,which then is exposed to the remaining portion of the catalyst bed asthe feed and effluent passed through the bed toward the reactor exit. Asthe depth of a catalyst bed is increased to provide longer run lengthbetween regeneration, a corresponding increase occurs in the amount ofsteaming that is performed on catalyst near the bottom of the bed. Thus,by the time that catalyst near the bottom of the bed starts toparticipate in oxygenate conversion, such catalyst can undergosubstantial deactivation due to catalyst steaming.

Using a plurality of moving bed reactors can reduce or minimize theimpact of both of the above types of catalyst deactivation. With regardto deactivation due to coking, the size of a moving bed reactor can beselected relative to the expected velocity of catalyst within the movingbed, so that the catalyst can be regenerated with a desired frequency.This can maintain coke on catalyst at less than a target level. Withregard to deactivation due to steaming, using a moving bed reactorsystem means that only the catalyst currently participating in aconversion or oligomerization reaction is exposed to steam. When notinside a moving bed reactor, the catalyst can be disengaged from theliquid phase and gas phase portions of the flow. Additionally, catalystcan be replaced at a convenient rate, so that the average steamingexposure of the catalyst is less than a target value. Thus, using aplurality of moving bed reactors can both reduce the amount of catalystexposure to steam relative to the amount of feed processed, and can alsoallow for control over the average steam exposure prior to replacementof the catalyst particles.

In this discussion, the “solids volume” within a reactor is defined asthe volume that receives solid catalyst particles to form the movingbed. In various aspects, the solid particles are introduced at or nearthe top of the solids volume, and form a cone at the angle of repose forthe solid particles. The solids volume includes the solids exit volume,where the mixture of solids, liquid, and any remaining gas are strippedfrom the solids using a stripping gas. In some aspects, the bottom ofthe solids exit volume corresponds to the bottom of the solids volume.In other aspects, the bottom of the solids volume can correspond to thebottom of the exit port(s) for the stripping gas used in the solids exitvolume.

In this discussion, the “reaction zone volume” corresponds to a regionwithin the solids volume. The top of the reaction zone volumecorresponds to the base of the cone that forms at the angle of repose inthe solids volume. The bottom of the reaction zone volume corresponds tothe beginning or top of the solids exit volume, where the solids arecontacted with stripping gas. The top of the solids exit volume can bedefined based on a change in the geometry, such as the transition from acylinder or annular shape to a cone shape, or the top of the solids exitvolume can correspond to the top of the exit port(s) for the strippinggas used in the solids exit volume.

In this discussion, operating a reactor to have a majority of the liquidtravel axially with the solid particles can be characterized based onone or more of the following features. In some aspects, 40 vol % or more(or 50 vol % or more) of the liquid that contacts the solid particles inthe reactor can be initially brought into contact with the solidparticles in the top 20% of the volume occupied by the solid particles,such as up to substantially all of the liquid. In other words,regardless of the length of the contact time with the particles, theinitial contact can be in the top 20% of the volume occupied by thesolid particles. In many aspects, this will have substantial overlapwith the top 20% of the solids volume, but the top 20% of the volumeoccupied by the solid particles can differ from the top 20% of thereaction zone volume in the reactor if there is substantial distancebetween the top level of the solid particles and the top of the reactor.By definition, any liquid that first comes into contact with a topsurface of the catalyst bed in the moving bed reactor corresponds toliquid that first contacts the top 20% of the volume occupied by thesolid particles.

Additionally or alternately, in some aspects 40 vol % or more (or 50 vol% or more) of the liquid that contacts the solid particles can beseparated from the solid particles in the bottom 20% of the volumeoccupied by the solid particles, such as up to substantially all of theliquid. In many aspects, this will have substantial overlap with thebottom 20% of the reactor volume, but the bottom 20% of the volumeoccupied by the solid particles can differ from the bottom 20% of thevolume in the reactor if there is substantial distance between thebottom level of the solid particles and the bottom of the reactorvolume.

It is noted that “top” and “bottom” are relative to the direction of theco-current flow of liquid and solid particles within the reactor. Invarious aspects, it can be convenient to align the direction of flowwith the direction of gravitational force, in order to reduce orminimize maldistribution of liquid relative to the solid particles dueto gravitational pull. However, if a reactor is oriented in anothermanner, the “top” and “bottom” of the solid particle bed can be definedso that the “top” corresponds to where solid particles are added to thebed and the “bottom” corresponds to where solid particles are removedfrom the bed (such as by exiting the reactor and passing into a transferpipe). It is noted that in an upflow configuration, this would result inthe “top” of the moving bed being closer to the bottom of the reactor,while the “bottom” of the moving bed would be closer to the top of thereactor.

In this discussion, operating a moving bed reactor with a three-phaseflow corresponds to operating a reactor where 45 vol %-70 vol %, or 50vol % to 70 vol % of the reaction zone volume corresponds to a solid(particles) phase; 10 vol % or more of the reactor volume corresponds toa liquid phase, such as 10 vol % to 45 vol %, or 20 vol % to 45 vol %,or 10 vol % to 35 vol %, or 20 vol % to 35 vol %, or 10 vol % to 30 vol%, or 10 vol % to 25 vol %; and 5 vol % or more of the reactor volumecorresponds to a gas phase, such as 5 vol % to 40 vol %, or 10 vol % to40 vol %, or 5 vol % to 35 vol %, or 5 vol % to 30 vol %, or 10 vol % to30 vol %, or 5 vol % to 25 vol %, or 5 vol % to 20 vol %.

In this discussion, fluid communication is defined as the ability forvapor and liquid to move between two process elements. Vaporcommunication is defined as the ability for vapor to move between twoprocess elements, while having reduced, limited, or optionally nomovement of liquid between such process elements. Solids flowcommunication is defined as the ability for solid particles to movebetween two process elements, which typically means that fluidcommunication is also possible.

Configuration Example 1—Example of Distributor Apparatus

FIG. 1 shows an example configuration for a distributor apparatus for amoving bed reactor. The distributor apparatus can be used for moving bedreactors where solids and liquids substantially travel through thereactor as an axial flow, while the gas flow can correspond to an axialflow, a radial flow, or any other convenient flow pattern. In someaspects, the distributor apparatus shown in FIG. 1 can be used inconjunction with a moving bed reactor where the catalyst is introducedalong the central axis of the reactor. This can result in the catalystfilling a central volume of the reactor. Such a configuration for amoving bed reactor can be suitable, for example, for a moving bedreactor where the catalyst, liquid, and gas all substantially traversethe reactor as axial flows. In other aspects, multiple instances of thedistributor apparatus in FIG. 1 can be arranged to provide catalyst foran annular catalyst volume in a moving bed reactor. This can bebeneficial for configurations such as the example shown in FIG. 4, wherethe catalyst and liquid in the moving bed reactor travel in asubstantially axial direction, while the gas in the feed contacts thecatalyst as a radial flow.

FIG. 1 shows a side view of an example of a distributor apparatus fordistribution of liquid when the solids are introduced along a centralaxis. In FIG. 1, a liquid distributor plate 101 is shown and highlightedwith hatch lines. The liquid distributor plate 101 fits into a movingbed reactor system through a system of connecting parts at the top andbottom of the distributor plate 101. The inlet feed pipes 102 areattached on the side of the top connecting part 103. Depending on theconfiguration, inlet feed pipes 102 can transport feed into the reactorin the form of gas, liquid, or a combination of gas and liquid. Forexample, in aspects where the gas portion of a feed contacts thecatalyst as a substantially radial flow, inlet feed pipes 102 cantransport a liquid portion of the feed into the reactor, withsubstantially all of the gas entering the reactor as a separate flow.

In FIG. 1, the catalyst particles enter the vessel through a solidsinlet conduit, such as catalyst feed line 104, which is attached in thecenter of the top connecting part 103. The distributor plate 101 sitsbelow the top connecting part 103. The portion of the feed provided byinlet pipes 102 drops into the distributor plate which includes one ormore concave shapes 105 with a radius R (shown in FIG. 2). There are anumber of slots (or orifices) 106 placed around the distributor plate.Preferably, the slots can be placed evenly and concentrically around thedistributor plate. The slots provide fluid communication between theconcave shape(s) 105 and a solids volume 108. As shown in FIG. 2, theseslots have a depth at the top 261 of the slots 106 and a depth at thebottom 262 of the slots 106. The slots can optionally be threaded onboth ends (i.e., at top 261 and at bottom 262) to allow installation ofnozzles at both the top and the bottom (not shown). The nozzles cancorrespond to, for example, hollow cylinders with an opening at the topto allow the passage of the gas. In some aspects, the nozzles canfurther include a slit around the top side of the nozzle. This can allowliquid to flow through once a certain liquid height is built. This willprevent selective distribution of the liquid through certain nozzles andallow an even flow of the liquid through all the nozzles. It is notedthat the nozzles at the bottom 262 of the slots 106 can have a geometrythat is selected to facilitate distribution of the expected type of feedthat is passing through the slots 106, such as nozzles selected fordistribution of gas, liquid, or a mixture of gas and liquid.

Depending on the aspect, solids volume 108 can correspond to a singlecentral volume, an annular volume, or another convenient volume thatallows for axial flow of catalyst and liquid through a moving bedreactor. In aspects where solids volume 108 corresponds to a centralvolume in a reactor, a single solids inlet conduit 104 can providecatalyst to the solids volume 108. As another example, in aspects wheresolids volume 108 corresponds to an annular volume, a plurality ofdistributor apparatus can be arranged in a substantially symmetricmanner around the solids volume 108. Such a configuration is shown inFIG. 4.

In the example of a distributor apparatus shown in FIGS. 1 and 2, thebottom of the distributor plate 101 curves toward the inside of thesolids volume at a 45 degree angle (or more generally an angle between30° and 55°). The gas and/or liquid will enter the nozzles inserted intothe distributor plate's slots (or orifices) 106 and first drop adistance prior to then curving inward, such as at angle 272, whichcorresponds to a 60 degree angle in FIG. 2 (or more generally an anglebetween 45° and 70°). The gas and/or liquid can then travel a furtherdistance to exit through another (bottom) set of nozzles inserted intoslots 106, as shown in FIG. 2. As shown in FIG. 1, the distributor platesits on top of the bottom connecting part 107 which has a form of afunnel whose bottom diameter is that of the solids volume 108 and topdiameter is that of the distributor plate. The top connecting part 103,the distributor plate 101, and the bottom connecting part 107 are heldtogether with a bolted clamp 109. The bottom connecting part 107 caneither be welded to the top of the reactor vessel 108, as shown in FIG.1, or bolted with a flange (not shown).

At the interface 120 between catalyst feed line (or other solids inletconduit) 104 and solids volume 108, a characteristic width of thecatalyst feed line 104 can be smaller than a characteristic width of thesolids volume that is receiving the catalyst. The characteristic widthof the catalyst feed line 104 corresponds to the longest straight linethat can be drawn between two points on the catalyst feed line at theinterface 120 with the solids volume 108. In aspects when the catalystfeed line is roughly cylindrical, the characteristic width will be thediameter of the catalyst feed line. The width of the solids volumereceiving the catalyst particles can correspond to a) for a centralvolume, the diameter of a cylindrical volume as measured at the locationwhere the base of the catalyst cone forms in the reactor; b) for anannular volume, the radial distance between the outer surface and theinner surface that define the annular volume, at the location where thebase of the catalyst cone forms in the annular volume; or c) a similarlycharacteristic width for a volume having a shape other than an annularvolume or a cylindrical volume.

It is noted that the above definitions for the width of the solidsvolume are based on the location of where the base of the catalyst coneforms. Above the base of the cone, there can typically be a gap betweenthe interface of the catalyst feed line with the solids volume and thebase of the catalyst cone. This gap, which can be referred to as acontact zone or mixing zone, corresponding to the difference between thetop of the solids volume and the top of the reaction zone volume, allowsthe catalyst cone to form at the angle of repose.

During operation, the solid (catalyst) particles exit the catalyst feedline 104 and distribute inside the solids volume 108, forming a conicalshape 110 whose angle corresponds to the angle of repose of the solidparticles. The conical shape 110 is formed in part because thecharacteristic width of the solids inlet conduit(s) is smaller than thewidth of the volume receiving the solid particles. The angle of reposefor solid particles can vary, such as having an angle of repose ofroughly 10° to 40°. The bottom inner edge of the feed distributor platewhere it meets the catalyst feed line bottom can be slightly angled,such as having an angle of 17° for angle 271, as shown in FIG. 2. Moregenerally, angle 271 can range from 10° to 25°. The gas or gas/liquidexiting the distributor plate through exit surface 279, via the bottomnozzles of slots 106, can inject directly on top of the cone ofparticles (at the angle of repose) formed by the flow of solid particlesinto the reactor. This will allow enhanced fluid mixing from the top andlet the fluid evenly disperse radially as it flows downward. This is duein part to the lateral velocity of the feed toward the central axis,which can assist with having feed well-mixed with particles throughoutthe reaction zone volume.

In FIG. 2, the complement of angle 272 is angle 273. Angle 273corresponds to an angle that the exit surface 279 makes relative to aplane defined by interface 120 between the catalyst feed line 104 andthe reactor vessel 108. In FIG. 2, angle 273 is shown as having a valueof 30°, but more generally angle 273 (i.e., the angle of the exitsurface relative to the plane) can have a value between roughly 15° and45°.

FIG. 3 shows the bottom of the distributor plate. In this schematicthere are 12 orifice nozzles at the top 261 and bottom 262. The offsetbetween the center of the top and bottom nozzles as the distributorplate curves inward toward the center of the reactor vessel can also beseen in this figure. In various aspects, the number of the nozzles canbe determined based on the scale of the reactor vessel, the optimumdistance needed to space the nozzles, and the liquid mass flux.

It is noted that the above description contemplates having a distributorapparatus that is machined as a separate part from other parts of theoverall reaction system. In other aspects, the distributor apparatus canbe integrated with the overall reaction system in any convenient manner.For example, the distribution plate can be attached to the catalyst feedline (or other solids inlet conduit) 104, so that there is no visiblejoint between catalyst feed line 104 and the distributor plate. In suchan aspect, the “opening” in the distributor plate that allows catalystto pass from feed line (or other solids inlet conduit) 104 to the solidsvolume 108 can correspond to a part of the solids inlet conduit 104. Itis noted that the attachment between catalyst feed line 104 and thedistributor plate can correspond to a removable attachment, or thatattachment can correspond to the catalyst feed line 104 and thedistributor plate corresponding to a single piece. Alternatively, thedistributor apparatus and catalyst feed line 104 can be separate pieces,with the catalyst feed line 104 passing through an opening in thedistributor apparatus.

Configuration Example 2—Reactor with Annular Catalyst Volume

FIG. 4 shows an example of a moving bed reactor suitable for performinga co-current reaction in the presence of three phases. The reactor inFIG. 4 is designed to introduce the catalyst and liquid into an annularvolume. The solid and liquid can flow axially through the annularvolume. The gas phase portion of the feed can then be passed through thecatalyst and liquid in a substantially radial direction.

In FIG. 4, reaction vessel 401 includes an outer annular volume 402 andan inner annular volume 403. The inner annular volume 403 is the annularregion where the catalyst or other solid particles reside, and thereforecan be referred to as an annular solids volume. The outer annular volume402 and inner annular volume 403 are arranged around a central doublepipe or conduit, corresponding to an outer central pipe or conduit 404and an inner central pipe or conduit 405. The inner annular volume 403can include perforations (not shown) that permit vapor communicationbetween the inner annular volume 403 and outer central pipe 404. Theperforations can primarily allow gas to pass into the outer central pipe404, but some liquid can also pass through the perforations. Theperforations are small enough to retain substantially all of the solidparticles in the annular solids volume 403.

During operation, gas is introduced into the reactor 401 via a centralopening 406 which connects to an inlet pipe 407 with openings fordistributing the gas into outer annular volume 402. The tops of innerannular volume 403, outer central pipe 404, and inner central pipe 405are sealed at the top, so that the flow path for gas to reach the outercentral pipe 404 is by passing radially through inner annular volume403. During operation, solid particles (such as catalyst particles) areintroduced into the reactor 401 via a plurality of pipes 408. Theoutlets of the plurality of pipes 408 are roughly centered over themid-point of inner annular volume 403. Similar to the configurationshown in FIG. 1, the solid particles fall into the inner annular volume403 and form cones 409 corresponding to the angle of repose for theparticles. The liquid phase is passed into reactor 401 via a pluralityof liquid conduits 410. The liquid conduits 410 feed a plurality ofslots or openings 411 that are arranged around the pipes 408.Optionally, the slots or openings 411 can include nozzles. Also similarto FIG. 1, the slots or openings 411 are arranged to cause the liquidfeed to impinge on the cones 409, in order to facilitate evendistribution of liquid within annular volume 403. Optionally butpreferably, the nozzles 411 can be oriented so that the liquid exitingfrom slots or openings 411 has a lateral velocity component. In someaspects, pipes 408 and liquid conduits 410 can have a similarrelationship to inner annular volume 403 as the relationships betweencatalyst inlet flow 104, inlet pipes 102, and solids volume 108. In suchaspects, liquid conduits 410 can be in fluid communication with annularvolume 403 via the plurality of slots or openings 411, in a mannersimilar to how inlet pipes 102 are in fluid communication with solidsvolume 108 via slots or openings 106.

During operation, gas from outer annular volume 402 passes radially intoinner annular volume 403. This allows contact between gas, liquid, andsolid for performing a desired reaction. The gas then continues radiallyinto the first or outer central pipe 404. Outer central pipe 404includes a plurality of bubble caps 412 or other structures that canallow gas to pass through into inner central pipe 405 while retainingliquid entrained with the gas in outer central pipe 404.

At the bottom of reactor 401, the gas, liquid, and solids can beseparated to allow for further processing and/or or for introductioninto a subsequent moving bed stage. The gas exits through a main gasexit line 416 that is in fluid communication with the bottom of innercentral pipe 405. The solids can exit from inner annular volume 403 intoa plurality of solids exit volumes, such as cone-shaped exit volumes 414as shown in FIG. 4. A stripping gas 415 is passed through the solidsexit volumes 414 to strip liquid from the solids prior to allowing thesolids to exit via solids exit line 418. It is noted that a baffle 419connects the cones 414, so that the stripping gas cannot bypass thecones. The stripping gas causes liquid in the solid particles to exitinto the bottom of first or outer central pipe 404, where it is combinedwith any liquid collected by the bubble caps 412. The liquid canaccumulate at the bottom of outer pipe 404 to a sufficient height sothat the liquid can exit through openings 413 into liquid exit line 417.

FIG. 5 shows a top view of the reactor 401 shown in FIG. 4. In FIG. 5,the input conduits corresponding to central opening 406, pipes 408 (fortransfer of solid particles), and liquid conduits 410 are shown inrelation to each other. It is noted that liquid conduits 410 are usedwithin the reactor to provide liquid to a plurality of nozzles 411 (notvisible in FIG. 5) that are arranged around each pipe 408.

It is noted that the configuration shown in FIG. 5 includes a total of 8solids inlet conduits 408 and two liquid conduits 410. More generally,any convenient number of solids inlet conduits 408 and liquid conduits410 can be used, so long as liquid is distributed around each solidsinlet conduit. For example, in the configuration shown in FIG. 5, adistributor plate can be used to distribute the liquid feed from liquidconduits 410 around each of the solids inlet conduits 408. This can beperformed by a single distributor plate that includes all of the liquidconduits 410 and solids inlet conduits 408. Alternatively, a part ofdistributor plates could be used, with each distributor plate receivingliquid from one liquid conduit 410 and distributing liquid to a portionof the solids inlet conduits 408. It is further noted that the annularsolids volume could be segmented using one or more internal walls. Thiscould allow a first group of solids inlet conduits 408 to providecatalyst particles to a first portion of the annular solids volume,while a second group of solids inlet conduits provides catalystparticles to a second portion of the annular solids volume. Moregenerally, any convenient number of portions could be defined in theannular solids volume.

Example of Reaction Conditions—Conversion of Oxygenates and/or Olefinsto Naphtha and Distillate

An example of the type of reaction that can be performed using the feeddistribution apparatus, feed separation method, and moving bed reactorsdescribed herein is conversion of oxygenates to olefins, optionally withfurther oligomerization of the olefins to naphtha and/or distillateboiling range products. Examples of suitable oxygenates include feedscontaining methanol, dimethyl ether, C₁-C₄ alcohols, ethers with C₁-C₄alkyl chains, including both asymmetric ethers containing C₁-C₄ alkylchains (such as methyl ethyl ether, propyl butyl ether, or methyl propylether) and symmetric ethers (such as diethyl ether, dipropyl ether, ordibutyl ether), or combinations thereof. It is noted that oxygenatescontaining at least one C₁-C₄ alkyl group are intended to explicitlyidentify oxygenates having alkyl groups containing 4 carbons or less.Preferably the oxygenate feed can include at least 30 wt % of one ormore suitable oxygenates, or at least 50 wt %, or at least 75 wt %, orat least 90 wt %, or at least 95 wt %. Additionally or alternately, theoxygenate feed can include at least 50 wt % methanol, such as at least75 wt % methanol, or at least 90 wt % methanol, or at least 95 wt %methanol. In particular, the oxygenate feed can include 30 wt % to 100wt % of oxygenate (or methanol), or 50 wt % to 95 wt %, or 75 wt % to100 wt %, or 75 wt % to 95 wt %. The oxygenate feed can be derived fromany convenient source. For example, the oxygenate feed can be formed byreforming of hydrocarbons in a natural gas feed to form synthesis gas(H₂, CO, CO₂), and then using the synthesis gas to form methanol (orother alcohols). As another example, a suitable oxygenate feed caninclude methanol, dimethyl ether, or a combination thereof as theoxygenate.

In addition to oxygenates, in some aspects the feed can also includeolefins. In this discussion, the olefins included as part of the feedcan correspond to aliphatic olefins that contain 6 carbons or less, sothat the olefins are suitable for formation of naphtha boiling rangecompounds. The olefin portion of the feed can be mixed with theoxygenates prior to entering a reactor for performing oxygenateconversion, or a plurality of streams containing oxygenates and/orolefins can be mixed within a conversion reactor. The feed can include 5wt % to 40 wt % of olefins (i.e., olefins containing 6 carbons or less),or 5 wt % to 30 wt %, or 10 wt % to 40 wt %, or 10 wt % to 30 wt %. Whenthe conversion is operated under low hydrogen transfer conditions with acatalyst that is selective for formation of paraffins and olefins, theaddition of olefins can allow for further production of paraffins andolefins. In aspects where olefins are included in the feed, the molarratio of oxygenates to olefins can be 20 or less, or 10 or less, or 6.0or less, or 4.0 or less, such as down to a molar ratio of 1.0. Forexample, the molar ratio of oxygenates to olefins can be between 1.0 and20, or between 1.0 and 10, or between 1.0 and 6.0, or between 4.0 and20, or between 6.0 and 20. It is noted that the weight percent ofolefins in the feed can be dependent on the nature of the olefins. Forexample, if a C₅ olefin is used as the olefin with a methanol-containingfeed, the wt % of olefin required to achieve a desired molar ratio ofolefin to oxygenate will be relatively high due to the much largermolecular weight of a C₅ alkene.

In some aspects, the olefins can correspond to olefins generated duringthe oxygenate conversion process. In such aspects, a portion of theeffluent from the conversion process can be recycled to provide olefinsfor the feed. In other aspects, the olefins can be derived from anyother convenient source. The olefin feed can optionally includecompounds that act as inerts or act as a diluent in the conversionprocess. For example, a stream of “waste” olefins having an olefincontent of 5 vol % to 20 vol % can be suitable as a source of olefins,so long as the other components of the “waste” olefins stream arecompatible with the conversion process. For example, the othercomponents of the olefin stream can correspond to inert gases such asN₂, carbon oxides, paraffins, and/or other gases that have lowreactivity under the conversion conditions. Water can also be present,although it can be preferable for water to correspond to 20 vol % orless of the total feed, or 10 vol % or less.

In addition to oxygenates and olefins, a feed can also include diluents,such as water (in the form of steam), nitrogen or other inert gases,and/or paraffins or other non-reactive hydrocarbons. In some aspects,the source of olefins can correspond to a low purity source of olefins,so that the source of olefins corresponds to 20 wt % or less of olefins.In some aspects, the portion of the feed corresponding to componentsdifferent from oxygenates and olefins can correspond to 1 wt % to 60 wt% of the feed, or 1 wt % to 25 wt %, or 10 wt % to 30 wt %, or 20 wt %to 60 wt %. Optionally, the feed can substantially correspond tooxygenates and olefins, so that the content of components different fromoxygenates and olefins is 1 wt % or less (such as down to 0 wt %).

It is noted that the above feed description can correspond to the inputstream for a group of moving bed reactors that are operated in series.In such aspects, the above feed can be passed into a first moving bedreactor, which partially converts oxygenates and/or partiallyoligomerizes olefins. The effluent from the first moving bed reactor canthen be separated into solid particles, gas phase unreacted feed andintermediate products, and liquid products (if any) that have formed.The solid particles, liquid, and gas can then be introduced into asecond moving bed reactor for further reaction. This can be repeateduntil a sufficient number of moving bed reactor stages have been used toachieve desired products. This can correspond to, for example, asufficient number of stages to achieve complete oxygenate conversion, asufficient number of stages so that oligomerization results in a desiredweight percentage (relative to the feed) of distillate boiling rangeproducts, or another convenient reaction end point.

In various aspects, the net yield of C₅₊ hydrocarbons in the conversioneffluent can be 10 wt % to 90 wt %, or 20 wt % to 80 wt %, or 40 wt % to90 wt %, or 40 wt % to 80 wt % on a dry basis. The conversion effluentcan correspond to the effluent from the final moving bed stage of aseries of moving bed reactors. The net yield refers to the yield of C₅₊hydrocarbons in the conversion effluent minus the amount (if any) of C₅₊alkenes in the feed. For example, when pentene is used as an olefin inthe feed, the weight of pentene in the feed is subtracted from theweight of C₅₊ hydrocarbons in the conversion effluent when determiningnet yield. It is noted that the net yield is expressed on a dry basisdue to the high variability in the amount of water that may be produced,depending on the oxygenate used as the feed. For example, if apre-conversion stage is used to convert methanol to water so thatdimethyl ether is used as a feed introduced into the moving bedreactors, the weight of water in the conversion effluent can be reducedby roughly 50 wt %. In various aspects, the yield of paraffins plusolefins relative to the C₅₊ portion of the hydrocarbon product can be 20wt % to 90 wt %, or 40 wt % to 90 wt %, or 40 wt % to 80 wt %.Additionally or alternately, less than 10 wt % of the total hydrocarbonproduct can correspond to C₁ paraffins (methane).

The total hydrocarbon product in the conversion effluent can include anaphtha boiling range portion, a distillate fuel boiling range portion,and a light ends portion. Optionally but preferably, the conversioneffluent can include 20 wt % or more of compounds boiling above thenaphtha boiling range (204° C.+), or 30 wt % or more.

Suitable and/or effective conditions for performing a conversionreaction and/or combined conversion plus oligomerization (i.e.upgrading) can include average reaction temperatures of 230° C. to 450°C., or 230° C. to 300° C., or 250° C. to 450° C., or 250° C. to 300° C.,or 300° C. to 450° C.; total pressures between 1 psig (˜7 kPag) to 400psig (˜2700 kPag), or 10 psig (˜70 kPag) to 150 psig (˜1050 kPag), or 10psig (˜70 kPag) to 100 psig (˜700 kPag), and an oxygenate space velocitybetween 0.1 hr⁻¹ to 10 hr⁻¹ based on weight of oxygenate relative toweight of catalyst (WHSV), or 0.1 hr⁻¹ to 5.0 hr⁻¹, or 1.0 hr⁻¹ to 5.0hr⁻¹. In this discussion, average reaction temperature is defined as theaverage of the temperature at the reactor inlet and the temperature atthe reactor outlet for the reactor where the conversion reaction isperformed.

In aspects where a separate series of moving bed reactors is used foroligomerization, suitable and/or effective conditions for performing anoligomerization reaction can include average reaction temperatures of180° C. to 250° C., or 200° C. to 250° C.; total pressures between 50psig (˜340 kPag) to 800 psig (˜5,500 kPag), and an oxygenate spacevelocity between 0.1 hr⁻¹ to 10 hr⁻¹ based on weight of oxygenaterelative to weight of catalyst (WHSV), or 0.1 hr⁻¹ to 5.0 hr⁻¹, or 1.0hr⁻¹ to 5.0 hr⁻¹.

In various aspects, a transition metal-enhanced zeolite catalystcomposition can be used for conversion of oxygenate feeds to naphthaboiling range fractions and olefins. In this discussion and the claimsbelow, a zeolite is defined to refer to a crystalline material having aporous framework structure built from tetrahedra atoms connected bybridging oxygen atoms. Examples of known zeolite frameworks are given inthe “Atlas of Zeolite Frameworks” published on behalf of the StructureCommission of the International Zeolite Association”, 6^(th) revisededition, Ch. Baerlocher, L. B. McCusker, D. H. Olson, eds., Elsevier,New York (2007) and the corresponding web site,http://www.iza-structure.ong/databases/. Under this definition, azeolite can refer to aluminosilicates having a zeolitic framework typeas well as crystalline structures containing oxides of heteroatomsdifferent from silicon and aluminum. Such heteroatoms can include anyheteroatom generally known to be suitable for inclusion in a zeoliticframework, such as gallium, boron, germanium, phosphorus, zinc, and/orother transition metals that can substitute for silicon and/or aluminumin a zeolitic framework.

A suitable zeolite can include a 1-dimensional or 2-dimensional10-member ring pore channel network. In some aspects, additionalbenefits can be achieved if the zeolite also has 12-member ring pocketsat the surface, such as MWW framework (e.g., MCM-49, MCM-22). Suchpockets represent active sites having a 12-member ring shape, but do notprovide access to a pore network. Examples of MWW framework zeolitesinclude MCM-22, MCM-36, MCM-49, MCM-56, EMM-10, EMM-12, EMM-13, andITQ-2. In some aspects, zeolites with a 1-dimensional or 2-dimensional12-member ring pore channel network can also be suitable, such as MORframework zeolites. Examples of suitable zeolites having a 1-dimensional10-member ring pore channel network include zeolites having a MRE (e.g,ZSM-48), MTW, TON (e.g., ZSM-22), MTT (e.g., ZSM-23), and/or MFSframework. In some aspects, ZSM-48, ZSM-22, MCM-22, MCM-49, or acombination thereof can correspond to preferred zeolites.

Generally, a zeolite having desired activity for methanol conversion canhave a silicon to aluminum molar ratio of 5 to 200, or 15 to 100, or 20to 80, or 20 to 40. For example, the silicon to aluminum ratio can be atleast 10, or at least 20, or at least 30, or at least 40, or at least50, or at least 60. Additionally or alternately, the silicon to aluminumratio can be 300 or less, or 200 or less, or 100 or less, or 80 or less,or 60 or less, or 50 or less.

It is noted that the molar ratio described herein is a ratio of siliconto aluminum. If a corresponding ratio of silica to alumina weredescribed, the corresponding ratio of silica (SiO₂) to alumina (Al₂O₃)would be twice as large, due to the presence of two aluminum atoms ineach alumina stoichiometric unit. Thus, a silicon to aluminum ratio of10 corresponds to a silica to alumina ratio of 20.

In some aspects, a zeolite in a catalyst can be present at least partlyin the hydrogen form. Depending on the conditions used to synthesize thezeolite, this may correspond to converting the zeolite from, forexample, the sodium form. This can readily be achieved, for example, byion exchange to convert the zeolite to the ammonium form followed bycalcination in air or an inert atmosphere at a temperature of 400° C. to700° C. to convert the ammonium form to the active hydrogen form.

Additionally or alternately, a zeolitic catalyst can include and/or beenhanced by a transition metal. The transition metal can be anyconvenient transition metal selected from Groups 6-15 of the IUPACperiodic table. The transition metal can be incorporated into thezeolite/catalyst by any convenient method, such as by impregnation, byion exchange, by mulling prior to extrusion, and/or by any otherconvenient method. Optionally, the transition metal incorporated into azeolite/catalyst can correspond to two or more metals. Afterimpregnation or ion exchange, the transition metal-enhanced catalyst canbe treated in air or an inert atmosphere at a temperature of 400° C. to700° C. The amount of transition metal can be expressed as a weightpercentage of metal relative to the total weight of the catalyst(including any zeolite and any binder). A catalyst can include 0.05 wt %to 20 wt % of one or more transition metals, or 0.1 wt % to 10 wt %, or0.1 wt % to 5 wt %, or 0.1 wt % to 2.0 wt %. For example, the amount oftransition metal can be at least 0.1 wt % of transition metal, or atleast 0.25 wt % of transition metal, or at least 0.5 wt %, or at least0.75 wt %, or at least 1.0 wt %. Additionally or alternately, the amountof transition metal can be 20 wt % or less, or 10 wt % or less, or 5 wt% or less, or 2.0 wt % or less, or 1.5 wt % or less, or 1.2 wt % orless, or 1.1 wt % or less, or 1.0 wt % or less.

A catalyst composition can employ a zeolite in its original crystallineform or after formulation into catalyst particles, such as by extrusion.A process for producing zeolite extrudates in the absence of a binder isdisclosed in, for example, U.S. Pat. No. 4,582,815, the entire contentsof which are incorporated herein by reference. Preferably, thetransition metal can be incorporated after formulation of the zeolite(such as by extrusion) to form catalyst particles without an addedbinder. Optionally, such an “unbound” catalyst can be steamed afterextrusion. The terms “unbound” is intended to mean that the presentcatalyst composition is free of any of the inorganic oxide binders, suchas alumina or silica, frequently combined with zeolite catalysts toenhance their physical properties.

The catalyst compositions described herein can further be characterizedbased on activity for hexane cracking, or Alpha value. Alpha value is ameasure of the acid activity of a zeolite catalyst as compared with astandard silica-alumina catalyst. The alpha test is described in U.S.Pat. No. 3,354,078; in the Journal of Catalysis, Vol. 4, p. 527 (1965);Vol. 6, p. 278 (1966); and Vol. 61, p. 395 (1980), each incorporatedherein by reference as to that description. The experimental conditionsof the test used herein include a constant temperature of 538° C. and avariable flow rate as described in detail in the Journal of Catalysis,Vol. 61, p. 395. Higher alpha values correspond with a more activecracking catalyst. For an oxygenate conversion catalyst, Alpha value canbe 15 to 150, or 15 to 100, or 15 to 50. Lower Alpha values can bebeneficial, as increased acidity can tend to increase hydrogen transfer.In other aspects, such as when the conversion is performed attemperatures of 275° C. or less, or 250° C. or less, catalysts with anAlpha value of 15 to 1000 can be suitable. This is due to thesuppression of hydrogen transfer at lower temperatures.

As an alternative to forming catalysts without a separate binder,zeolite crystals can be combined with a binder to form bound catalysts.Suitable binders for zeolite-based catalysts can include variousinorganic oxides, such as silica, alumina, zirconia, titania,silica-alumina, cerium oxide, magnesium oxide, yttrium oxide, orcombinations thereof. For catalysts including a binder, the catalyst cancomprise at least 10 wt % zeolite, or at least 30 wt %, or at least 50wt %, such as up to 90 wt % or more. Generally, a binder can be presentin an amount between 1 wt % and 90 wt %, for example between 5 wt % and40 wt % of a catalyst composition. In some aspects, the catalyst caninclude at least 5 wt % binder, such as at least 10 wt %, or at least 20wt %. Additionally or alternately, the catalyst can include 90 wt % orless of binder, such as 50 wt % or less, or 40 wt % or less, or 35 wt %or less. Combining the zeolite and the binder can generally be achieved,for example, by mulling an aqueous mixture of the zeolite and binder andthen extruding the mixture into catalyst pellets. A process forproducing zeolite extrudates using a silica binder is disclosed in, forexample, U.S. Pat. No. 4,582,815. Optionally, a bound catalyst can besteamed after extrusion.

ADDITIONAL EMBODIMENTS

Embodiment 1. A moving bed reactor, comprising: a reactor comprising anannular outer volume, an annular solids volume inside the annular outervolume, a first central conduit inside of the annular solids volume, andan inner central conduit inside the first central conduit, the annularsolids volume comprising a plurality of perforations providing vaporcommunication between the annular outer volume and the first centralconduit; a central gas opening in fluid communication with the outerannular volume; a plurality of solids inlet conduits in solids flowcommunication with the annular solids volume; one or more distributorplates comprising distributor plate concave volumes, a plurality of thedistributor plate concave volumes being arranged around each of thesolids inlet conduits, each distributor plate concave volume comprisingone or more orifices providing fluid communication between eachdistributor plate concave volume and the annular solids volume; aplurality of liquid inlet conduits in fluid communication with thedistributor plate concave volumes; a gas exit conduit in fluidcommunication with the inner central volume; a liquid exit conduit influid communication with the outer central volume; and a solids exitvolume in solids flow communication with a bottom of the solids annularvolume, the solids exit volume further comprising a stripping gas inletand a stripping gas outlet, the stripping gas outlet providing fluidcommunication with the outer central volume.

Embodiment 2. The reactor of Embodiment 1, wherein the one or moredistributor plates further comprise a plurality of exit surfacesseparating the distributor plate concave volumes from the annular solidsvolume, the one or more orifices providing fluid communication betweeneach concave volume and the annular solids volume through an exitsurface, and wherein the plurality of exit surfaces are oriented at anangle of 15° to 45° relative to a plane defined by at least oneinterface between the one or more solids inlet conduits and the solidsvolume.

Embodiment 3. The reactor of any of the above embodiments, wherein eachorifice further comprises a nozzle, the nozzle comprising a slit at aliquid level height.

Embodiment 4. The reactor of any of the above embodiments, wherein theplurality of solids inlet conduits have a smaller characteristic widththan a width of the solids volume at an interface between each solidsinlet conduit and the solids volume

Embodiment 5. The reactor of any of the above embodiments, wherein theperforations prevent flow of solid particles into the annular outervolume and into the first central conduit.

Embodiment 6. The reactor of any of the above embodiments, wherein theplurality to of solids inlet conduits provide solids flow communicationbetween a source of solid particles and the solids annular volume, thesource of solid particles comprising a solids exit volume of a secondmoving bed reactor, a regenerator, or a combination thereof.

Embodiment 7. The reactor of any of the above embodiments, wherein thereactor further comprises solid particles in the solids annular volume,a top surface of the solid particles forming a plurality of cones at theangle of repose for the solid particles.

Embodiment 8. The reactor of any of the above embodiments, wherein theplurality of solids inlet conduits pass through a plurality of openingsin the one or more distributor plates, or wherein the one or moredistributor plates comprise the plurality of solids inlet conduits.

Embodiment 9. A method for operating a moving bed reactor, comprising:passing solid particles into an annular solids volume of a moving bedreactor through a plurality of solids inlet conduits, the solidparticles forming a plurality of cones at an angle of repose for thesolid particles within the annular solids volume; passing a liquid feedinto the annular solids volume, at least a portion of the liquid feedimpinging on the plurality of cones formed by the solid particles;contacting the solid particles with a gas feed by passing the gas feedfrom an outer annular volume, through the annular solids volume, througha first central conduit, and into an inner central conduit; moving thesolid particles and a liquid effluent through the annular solids volumeinto a solids exit volume; stripping the liquid effluent from the solidparticles by passing a stripping gas through the solids exit volume andinto the first central conduit.

Embodiment 10. The method of Embodiment 9, wherein passing the liquidfeed into the annular solids volume comprises: introducing the liquidfeed into a plurality of concave volumes in a distributor plate, theplurality of concave volumes being arranged around each of the pluralityof solids inlet conduits, each concave volume comprising one or moreorifices, the one or more orifices providing fluid communication betweenthe plurality of concave volumes and the annular solids volume via aplurality of exit surfaces; and passing the liquid feed through the oneor more orifices into the annular solids volume, wherein the pluralityof exit surfaces are oriented at an angle of 15° to 45° relative to aplane defined by at least one interface between the plurality of solidsinlet conduits and the annular solids volume.

Embodiment 11. The method of Embodiment 9 or 10, wherein the at least aportion of the liquid feed comprises a lateral velocity component as itimpinges on the plurality of cones, or wherein the at least a portion ofthe liquid feed comprises 40 vol % or more of the volume of the liquidfeed, or a combination thereof.

Embodiment 12. The method of any of Embodiments 9 to 11, wherein theliquid effluent comprises 50 vol % or more of a volume of the liquidfeed.

Embodiment 13. The method of any of Embodiments 9 to 12, wherein theliquid effluent comprises at least one liquid reaction product formed bycontacting the solid particles with the liquid feed, the gas feed, or acombination thereof.

Embodiment 14. The method of any of Embodiments 9 to 13, wherein theplurality of solids inlet conduits provide solids flow communicationbetween a source of solid particles and the solids annular volume, thesource of solid particles comprising a solids exit volume of a secondmoving bed reactor, a regenerator, or a combination thereof.

Embodiment 15. A liquid effluent formed using the reactor of any ofEmbodiments 1 to 8 or formed according to the method of any ofEmbodiments 9 to 14.

While the present invention has been described and illustrated byreference to particular embodiments, those of ordinary skill in the artwill appreciate that the invention lends itself to variations notnecessarily illustrated herein. For this reason, then, reference shouldbe made solely to the appended claims for purposes of determining thetrue scope of the present invention.

The invention claimed is:
 1. A moving bed reactor, comprising: a reactor comprising an annular outer volume, an annular solids volume inside the annular outer volume, a first central conduit inside of the annular solids volume, and an inner central conduit inside the first central conduit, the annular solids volume comprising a plurality of perforations providing vapor communication between the annular outer volume and the first central conduit; a central gas opening in fluid communication with the outer annular volume; a plurality of solids inlet conduits in solids flow communication with the annular solids volume; one or more distributor plates comprising distributor plate concave volumes, a plurality of the distributor plate concave volumes being arranged around each of the solids inlet conduits, each distributor plate concave volume comprising one or more orifices providing fluid communication between each distributor plate concave volume and the annular solids volume; a plurality of liquid inlet conduits in fluid communication with the distributor plate concave volumes; a gas exit conduit in fluid communication with the inner central volume; a liquid exit conduit in fluid communication with the outer central volume; and a solids exit volume in solids flow communication with a bottom of the solids annular volume, the solids exit volume further comprising a stripping gas inlet and a stripping gas outlet, the stripping gas outlet providing fluid communication with the outer central volume.
 2. The reactor of claim 1, wherein the one or more distributor plates further comprise a plurality of exit surfaces separating the distributor plate concave volumes from the annular solids volume, the one or more orifices providing fluid communication between each concave volume and the annular solids volume through an exit surface.
 3. The reactor of claim 2, wherein the plurality of exit surfaces are oriented at an angle of 15° to 45° relative to a plane defined by at least one interface between the one or more solids inlet conduits and the solids volume.
 4. The reactor of claim 1, wherein each orifice further comprises a nozzle, the nozzle comprising a slit at a liquid level height.
 5. The reactor of claim 1, wherein the plurality of solids inlet conduits have a smaller characteristic width than a width of the solids volume at an interface between each solids inlet conduit and the solids volume.
 6. The reactor of claim 1, wherein the perforations prevent flow of solid particles into the annular outer volume and into the first central conduit.
 7. The reactor of claim 1, wherein the plurality of solids inlet conduits provide solids flow communication between a source of solid particles and the solids annular volume.
 8. The reactor of claim 7, wherein the source of solid particles comprises a solids exit volume of a second moving bed reactor, a regenerator, or a combination thereof.
 9. The reactor of claim 1, wherein the reactor further comprises solid particles in the solids annular volume, a top surface of the solid particles forming a plurality of cones at the angle of repose for the solid particles.
 10. The reactor of claim 1, wherein the plurality of solids inlet conduits pass through a plurality of openings in the one or more distributor plates, or wherein the one or more distributor plates comprise the plurality of solids inlet conduits.
 11. The reactor of claim 1, wherein the central gas opening comprises an opening in a distributor plate of the one or more distributor plates.
 12. A method for operating a moving bed reactor, comprising: passing solid particles into an annular solids volume of a moving bed reactor through a plurality of solids inlet conduits, the solid particles forming a plurality of cones at an angle of repose for the solid particles within the annular solids volume; passing a liquid feed into the annular solids volume, at least a portion of the liquid feed impinging on the plurality of cones formed by the solid particles; contacting the solid particles with a gas feed by passing the gas feed from an outer annular volume, through the annular solids volume, through a first central conduit, and into an inner central conduit; moving the solid particles and a liquid effluent through the annular solids volume into a solids exit volume; stripping the liquid effluent from the solid particles by passing a stripping gas through the solids exit volume and into the first central conduit.
 13. The method of claim 12, wherein passing the liquid feed into the annular solids volume comprises: introducing the liquid feed into a plurality of concave volumes in a distributor plate, the plurality of concave volumes being arranged around each of the plurality of solids inlet conduits, each concave volume comprising one or more orifices, the one or more orifices providing fluid communication between the plurality of concave volumes and the annular solids volume via a plurality of exit surfaces; and passing the liquid feed through the one or more orifices into the annular solids volume.
 14. The method of claim 13, wherein the plurality of exit surfaces are oriented at an angle of 15° to 45° relative to a plane defined by at least one interface between the plurality of solids inlet conduits and the annular solids volume.
 15. The method of claim 12, wherein the at least a portion of the liquid feed comprises a lateral velocity component as it impinges on the plurality of cones.
 16. The method of claim 12, wherein the liquid effluent comprises 50 vol % or more of a volume of the liquid feed.
 17. The method of claim 12, wherein the liquid effluent comprises at least one liquid reaction product formed by contacting the solid particles with the liquid feed, the gas feed, or a combination thereof.
 18. The method of claim 12, wherein the at least a portion of the liquid feed comprises 40 vol % or more of the volume of the liquid feed.
 19. The method of claim 12, wherein the plurality of solids inlet conduits provide solids flow communication between a source of solid particles and the solids annular volume.
 20. The method of claim 19, wherein the source of solid particles comprises a solids exit volume of a second moving bed reactor, a regenerator, or a combination thereof. 